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USGS2008

A comparison of winter mercury accumulation at forested and no-canopy sites measured with different snow sampling techniques

Atmospheric mercury (Hg) is delivered to ecosystems via rain, snow, cloud/fog, and dry deposition. The importance of snow, especially snow that has passed through the forest canopy (throughfall), in delivering Hg to terrestrial ecosystems has received little attention in the literature. The snowpack is a dynamic system that links atmospheric deposition and ecosystem cycling through deposition and emission of deposited Hg. To examine the magnitude of Hg delivery via snowfall, and to illuminate processes affecting Hg flux to catchments during winter (cold season), Hg in snow in no-canopy areas and under forest canopies measured with four collection methods were compared: (1) Hg in wet precipitation as measured by the Mercury Deposition Network (MDN) for the site in Acadia National Park, Maine, USA, (2) event throughfall (collected after snowfall cessation for accumulations of >8 cm), (3) season-long throughfall collected using the same apparatus for event sampling but deployed for the entire cold season, and (4) snowpack sampling. Estimates (mean ± SE) of Hg deposition using these methods during the 91-day cold season in 2004–2005 at conifer sites showed that season-long throughfall Hg flux (1.80 μg/m 2 ) < snowpack Hg (2.38 ± 0.68 μg/m 2 ) < event throughfall flux (5.63 ± 0.38 μg/m 2 ). Mercury deposition at the MDN site (0.91 μg/m 2 ) was similar to that measured at other no-canopy sites in the area using the other methods, but was 3.4 times less than was measured under conifer canopies using the event sampling regime. This indicates that snow accumulated under the forest canopy received Hg from the overstory or exhibited less re-emission of Hg deposited in snow relative to open areas. The soil surface of field-scale plots were sprayed with a natural rain water sample that contained an Hg tracer ( 202 Hg) just prior to the first snowfall to explore whether some snowpack Hg might be explained from soil emissions. The appearance of the 202 Hg tracer in the snowpack (0–64% of the total Hg mass in the snowpack) suggests that movement of Hg from the soil into the snowpack is possible. However, as with any tracer study the 202 Hg tracer may not precisely represent the reactivity and mobility of natural Hg in soils.

Applied Geochemistry↗

USGS2012

Acidification of Earth: An assessment across mechanisms and scales

In this review article, anthropogenic activities that cause acidification of Earth’s air, waters, and soils are examined. Although there are many mechanisms of acidification, the focus is on the major ones, including emissions from combustion of fossil fuels and smelting of ores, mining of coal and metal ores, and application of nitrogen fertilizer to soils, by elucidating the underlying biogeochemical reactions as well as assessing the magnitude of the effects. These widespread activities have resulted in (1) increased CO 2 concentration in the atmosphere that acidifies the oceans; (2) acidic atmospheric deposition that acidifies soils and bodies of freshwater; (3) acid mine drainage that acidifies bodies of freshwater and groundwaters; and (4) nitrification that acidifies soils. Although natural geochemical reactions of mineral weathering and ion exchange work to buffer acidification, the slow reaction rates or the limited abundance of reactant phases are overwhelmed by the onslaught of anthropogenic acid loading. Relatively recent modifications of resource extraction and usage in some regions of the world have begun to ameliorate local acidification, but expanding use of resources in other regions is causing environmental acidification in previously unnoticed places. World maps of coal consumption, Cu mining and smelting, and N fertilizer application are presented to demonstrate the complex spatial heterogeneity of resource consumption as well as the overlap in acidifying potential derived from distinctly different phenomena. Projected population increase by country over the next four decades indicates areas with the highest potential for acidification, so enabling anticipation and planning to offset or mitigate the deleterious environmental effects associated with these global shifts in the consumption of energy, mineral, and food resources.

Applied Geochemistry↗

USGS2012

Surface heat flow and CO2 emissions within the Ohaaki hydrothermal field, Taupo Volcanic Zone, New Zealand

Carbon dioxide emissions and heat flow have been determined from the Ohaaki hydrothermal field, Taupo Volcanic Zone (TVZ), New Zealand following 20 a of production (116 MW e ). Soil CO 2 degassing was quantified with 2663 CO 2 flux measurements using the accumulation chamber method, and 2563 soil temperatures were measured and converted to equivalent heat flow (W m −2 ) using published soil temperature heat flow functions. Both CO 2 flux and heat flow were analysed statistically and then modelled using 500 sequential Gaussian simulations. Forty subsoil CO 2 gas samples were also analysed for stable C isotopes. Following 20 a of production, current CO 2 emissions equated to 111 ± 6.7 T/d. Observed heat flow was 70 ± 6.4 MW, compared with a pre-production value of 122 MW. This 52 MW reduction in surface heat flow is due to production-induced drying up of all alkali–Cl outflows (61.5 MW) and steam-heated pools (8.6 MW) within the Ohaaki West thermal area (OHW). The drying up of all alkali–Cl outflows at Ohaaki means that the soil zone is now the major natural pathway of heat release from the high-temperature reservoir. On the other hand, a net gain in thermal ground heat flow of 18 MW (from 25 MW to 43.3 ± 5 MW) at OHW is associated with permeability increases resulting from surface unit fracturing by production-induced ground subsidence. The Ohaaki East (OHE) thermal area showed no change in distribution of shallow and deep soil temperature contours despite 20 a of production, with an observed heat flow of 26.7 ± 3 MW and a CO 2 emission rate of 39 ± 3 T/d. The negligible change in the thermal status of the OHE thermal area is attributed to the low permeability of the reservoir beneath this area, which has limited production (mass extraction) and sheltered the area from the pressure decline within the main reservoir. Chemistry suggests that although alkali–Cl outflows once contributed significantly to the natural surface heat flow (∼50%) they contributed little (<1%) to pre-production CO 2 emissions due to the loss of >99% of the original CO 2 content due to depressurisation and boiling as the fluids ascended to the surface. Consequently, the soil has persisted as the major (99%) pathway of CO 2 release to the atmosphere from the high temperature reservoir at Ohaaki. The CO 2 flux and heat flow surveys indicate that despite 20 a of production the variability in location, spatial extent and magnitude of CO 2 flux remains consistent with established geochemical and geophysical models of the Ohaaki Field. At both OHW and OHE carbon isotopic analyses of soil gas indicate a two-stage fractionation process for moderate-flux (>60 g m −2 d −1 ) sites; boiling during fluid ascent within the underlying reservoir and isotopic enrichment as CO 2 diffuses through porous media of the soil zone. For high-flux sites (>300 g m −2 d −1 ), the δ 13 CO 2 signature (−7.4 ± 0.3‰ OHW and −6.5 ± 0.6‰ OHE) is unaffected by near-surface (soil zone) fractionation processes and reflects the composition of the boiled magmatic CO 2 source for each respective upflow. Flux thresholds of <30 g m −2 d −1 for purely diffusive gas transport, between 30 and 300 g m −2 d −1 for combined diffusive–advective transport, and ⩾300 g m −2 d −1 for purely advective gas transport at Ohaaki were assigned. δ 13 CO 2 values and cumulative probability plots of CO 2 flux data both identified a threshold of ∼15 g m −2 d −1 by which background (atmospheric and soil respired) CO 2 may be differentiated from hydrothermal CO 2 .

Taupo Volcanic Zone↗

USGS2013

Tracing groundwater with low-level detections of halogenated VOCs in a fractured carbonate-rock aquifer, Leetown Science Center, West Virginia, USA

Measurements of low-level concentrations of halogenated volatile organic compounds (VOCs) and estimates of groundwater age interpreted from 3 H/ 3 He and SF 6 data have led to an improved understanding of groundwater flow, water sources, and transit times in a karstic, fractured, carbonate-rock aquifer at the Leetown Science Center (LSC), West Virginia. The sum of the concentrations of a set of 16 predominant halogenated VOCs (TDVOC) determined by gas chromatography with electron-capture detector (GC–ECD) exceeded that possible for air–water equilibrium in 34 of the 47 samples (median TDVOC of 24,800 pg kg −1 ), indicating that nearly all the water sampled in the vicinity of the LSC has been affected by addition of halogenated VOCs from non-atmospheric source(s). Leakage from a landfill that was closed and sealed nearly 20 a prior to sampling was recognized and traced to areas east of the LSC using low-level detection of tetrachloroethene (PCE), methyl chloride (MeCl), methyl chloroform (MC), dichlorodifluoromethane (CFC-12), and cis-1,2-dichloroethene (cis-1,2-DCE). Chloroform (CHLF) was the predominant VOC in water from domestic wells surrounding the LSC, and was elevated in groundwater in and near the Fish Health Laboratory at the LSC, where a leak of chlorinated water occurred prior to 2006. The low-level concentrations of halogenated VOCs did not exceed human or aquatic-life health criteria, and were useful in providing an awareness of the intrinsic susceptibility of the fractured karstic groundwater system at the LSC to non-atmospheric anthropogenic inputs. The 3 H/ 3 He groundwater ages of spring discharge from the carbonate rocks showed transient behavior, with ages averaging about 2 a in 2004 following a wet climatic period (2003–2004), and ages in the range of 4–7 a in periods of more average precipitation (2008–2009). The SF 6 and CFC-12 data indicate older water (model ages of 10s of years or more) in the low-permeability shale of the Martinsburg Formation located to the west of the LSC. A two-a record of specific conductance, water temperature, and discharge recorded at 30-min intervals demonstrated an approximately 3-month lag in discharge at Gray Spring. The low groundwater ages of waters from the carbonate rocks support rapid advective transport of contaminants from the LSC vicinity, yet the nearly ubiquitous occurrence of low-level concentrations of halogenated VOCs at the LSC suggests the presence of long-term persistent sources, such as seepage from the closed and sealed landfill, infiltration of VOCs that may persist locally in the epikarst, exchange with low-permeability zones in fractured rock, and upward leakage of older water that may contain elevated concentrations of halogenated VOCs from earlier land use activities.

West Virginia↗

USGS2009

Modeling Carbon Dioxide, pH and Un-Ionized Ammonia Relationships in Serial Reuse Systems

In serial reuse systems, excretion of metabolic carbon dioxide has a significant impact on ambient pH, carbon dioxide, and un-ionized ammonia concentrations. This impact depends strongly on alkalinity, water flow rate, feeding rate, and loss of carbon dioxide to the atmosphere. A reduction in pH from metabolic carbon dioxide can significantly reduce the un-ionized ammonia concentration and increase the carbon dioxide concentrations compared to those parameters computed from influent pH. The ability to accurately predict pH in serial reuse systems is critical to their design and effective operation. A trial and error solution to the alkalinity–pH system was used to estimate important water quality parameters in serial reuse systems. Transfer of oxygen and carbon dioxide across the air–water interface, at overflow weirs, and impacts of substrate-attached algae and suspended bacteria were modeled. Gas transfer at the weirs was much greater than transfer across the air–water boundary. This simulation model can rapidly estimate influent and effluent concentrations of dissolved oxygen, carbon dioxide, and un-ionized ammonia as a function of water temperature, elevation, water flow, and weir type. The accuracy of the estimates strongly depends on assumed pollutional loading rates and gas transfer at the weirs. The current simulation model is based on mean daily loading rates; the impacts of daily variation loading rates are discussed. Copies of the source code and executable program are available free of charge.

Aquacultural Engineering↗

USGS2005

Evaluation of argon ages and integrity of fluid-inclusion compositions: Stepwise noble gas heating experiments on 1.87 Ga alunite from Tapajós Province, Brazil

Quantitative analyses are reported for active (N 2 , CH 4 , CO, CO 2 , H 2 , O 2 , HF, HCl, H 2 S, SO 2 ) and noble (He, Ar, Ne) gases released by crushing and step heating of magmatic-hydrothermal alunite from the Tapajós gold province in Brazil. This is the oldest known alunite ( 40 Ar/ 39 Ar age of 1.87 Ga), and because it has undergone minimal postdepositional thermal or tectonic strain, it is excellent material to test the retention of gas species in fluid inclusions and within the crystal structure over geological time. The gas compositions of a single sample, in combination with Ar age-spectrum data derived from stepwise heating of 10 related samples, have been used to constrain the limits of modification of primary gas compositions in fluid inclusions and the possible extent of the loss of radiogenic Ar. The observed variations in the isotopic compositions of He, Ne, and Ar released by stepwise heating have been used to identify the residence sites and determine the diffusion coefficients of the gases in the mineral. The data suggest that the only modification to primary gas compositions after entrapment in fluid inclusions and formation of the mineral is due to radiogenic and nucleogenic processes which affect the noble gas isotopic compositions. Three gas retention sites are recognized in alunite: (1) primary fluid inclusions, (2) crystal structure OH sites, and (3) crystal structure sulfate sites. Alunite undergoes OH loss at <500°C, and K-SO 4 structural decomposition occurs at >600°C. Fluid inclusions generally are ≤1 μm in diameter and have variable but high vapor/liquid ratios. The gases in inclusion fluids are quantitatively released in vacuo by heating at 200°C for &sim;1 h. In the inclusion fluids, H 2 O is 32 mol% of total gas, H 2 S/SO 2 ranges from approximately 4 to 2, and N 2 /Ar from 0.3 to 96.3. The presence of large amounts of H 2 and CO indicates disequilibrium among the gas species in the fluids. Helium abundance is 214 ppm. Helium from fluid inclusions ( R /Ra=19.5) makes up about 4% of the total helium, whereas He ( R /Ra=0.2–2.0) from the crystal structure makes up about 65% of the total. Argon from fluid inclusions has 40 Ar/ 36 Ar=584–629 and that from crystal structure sites is >9.6×10 4 . Most gases are released from fluid inclusions at 200 °C, whereas most Ar (≥95%) is released between 525 and 725°C. Argon released from fluid inclusions at 200°C has 38 Ar/ 36 Ar=0.0–0.064. In contrast, Ar released from the matrix of the mineral at high temperature has 38 Ar/ 36 Ar=3.6–14.7. This difference suggests that, since the formation of the alunite at 1.87 Ga, traces of Cl in the mineral structure have undergone Cl ( n , γ ) and 41 K ( n , α ) in situ reactions with neutrons derived from U–Th. The amount of 36 Ar production from Cl nucleogenic reactions used in correcting for atmospheric 40 Ar typically increases the calculated age by 1–5 m.y., which is generally an insignificant component of the determined Ar age. Decay of U–Th over this time contributes 4 He ( α ) buildup in the crystal structure K-SO 4 sites. Atmospheric corrected excess 21 Ne/ 22 Ne=0.028–0.409 indicates that nucleogenic Ne was also produced via ( α , n ) reactions in matrix sites. Diffusion coefficients and activation energies for the diffusion of Ar and He, as determined using Arrhenius plots, indicate two distinct groups definable by their differences in activation energies. Argon log D o =2.45 and 15.33, with activation energies of 225 and 465 kJ mol −1 , respectively; the diffusion of He in alunite is quantified with log D o =−4.33 and E =106.8 kJ mol −1 . Model calculations of simplistic 1/ e -folding times and diffusion distance–time curves indicate that He should remain in alunite for millions of years at ≤100°C, whereas at <200–220°C, the alunite will retain Ar almost indefinitely. The data demonstrate why alunite is suitable for Ar geochronological applications and also show that, unless the alunite is subjected to metamorphic deformation, the inclusion fluids should retain their primary compositions.

Tapajós Province↗

USGS2005

Characterization of gas chemistry and noble-gas isotope ratios of inclusion fluids in magmatic-hydrothermal and magmatic-steam alunite

Chemical and isotope data were obtained for the active gas and noble gas of inclusion fluids in coarse-grained samples of magmatic-hydrothermal and magmatic-steam alunite from well-studied deposits (Marysvale, Utah; Tambo, Chile; Tapajo??s, Brazil; Cactus, California; Pierina, Peru), most of which are discussed in this Volume. Primary fluid inclusions in the alunite typically are less than 0.2 ??m but range up to several micrometers. Analyses of the active-gas composition of these alunite-hosted inclusion fluids released in vacuo by both crushing and heating indicate consistent differences in the compositions of magmatic-hydrothermal and magmatic-steam fluids. The compositions of fluids released by crushing were influenced by contributions from significant populations of secondary inclusions that trapped largely postdepositional hydrothermal fluids. Thermally released fluids gave the best representation of the fluids that formed primary alunite. The data are consistent with current models for the evolution of magmatic-hydrothermal and magmatic-steam fluids. Magmatic-steam fluids are vapor-dominant, average about 49 mol% H2O, and contain N2, H2, CH4, CO, Ar, He, HF, and HCl, with SO2 the dominant sulfur gas (average SO2/ H2S=202). In contrast, magmatic-hydrothermal fluids are liquid-dominant, average about 88 mol% H2O, and N2, H2, CO2, and HF, with H2S about as abundant as SO2 (average SO2/H2 S=0.7). The low SO2/H2S and N2/Ar ratios, and the near-absence of He in magmatic-hydrothermal fluids, are consistent with their derivation from degassed condensed magmatic fluids whose evolution from reduced-to-oxidized aqueous sulfur species was governed first by rock and then by fluid buffers. The high SO2/H2S and N2/Ar with significant concentrations of He in magmatic-steam fluids are consistent with derivation directly from a magma. None of the data supports the entrainment of atmospheric gases or mixing of air-saturated gases in meteoric water in either magmatic-hydrothermal or magmatic-steam fluids. Thus, the oxidation of SO2 to aqueous sulfate in the magmatic-steam fluids did not result from mixing with atmospheric oxygen. Both of the fluid types are characterized by high H2 contents that range from 0.2 mol% to the extraordinarily large amounts (66 mol%) observed in some magmatic-steam fluids. Modeling of gas speciation using SOLVGAS requires most of the gas species to have been in disequilibrium at the time of their trapping in the fluid inclusions. The origin of such extreme H2 concentrations, although problematic, is thought to be largely related to accumulation of H2 from the reaction of water with ferrous iron during the rise of magma and probably even after exsolution of fluid from a magma. The large contents of reduced gases in the inclusion fluids are far in excess of those observed in volcanic emanations, and are thought to reflect the close "sampling position" of the host alunite relative to the location of the magma. Isotope ratios of He and Ne indicate largely crustal sources for these gases in the alunite parental fluids derived from Tertiary magmas, but a greater mantle component for the gases in alunite parental fluids derived from Proterozoic magmas.

Chemical Geology↗

USGS2007

High arsenic concentrations and enriched sulfur and oxygen isotopes in a fractured-bedrock ground-water system

Ground water with high arsenic concentrations (up to 26.6????mol L- 1) has sulfate enriched in 34S and 18O in the fractured-bedrock, ground-water system of the Kelly's Cove watershed, Northport, Maine, USA. The ranges of sulfur and oxygen isotope values in aqueous sulfate, ??34S[SO4] and ??18O[SO4], at the Kelly's Cove watershed are + 3.4 to + 4.9??? and - 2.0 to + 6.7???, respectively. These isotope values are strikingly similar to those of the Goose River, Maine watershed which has ??34S[SO4] and ??18O[SO4] ranges of + 3.7 to + 4.6 ??? and - 2.6 to + 7.5???, respectively. In both systems, high arsenic concentrations occur with high ??34S[SO4] and ??18O[SO4] values, yet redox conditions and underlying rock types are quite different. The isotope values of sulfide minerals, ??34S[min], from four bedrock cores vary over short distances and range from - 5.1 to + 7.5???. The ??34S[SO4] values are controlled by the ??34S[min] values with minor input of atmospheric SO4. The much narrower range in ??34S[SO4] values than ??34S[min] values is probably due to sufficient ground-water mixing at a scale greater than the ??34S[min] variability. The ??34S[SO4] values are about 2??? higher than the average ??34S[min] value and fall within the range of ??34S[min] values, indicating only minor fractionation due to bacterial reduction of SO4. The highest ??18O[SO4] values were measured in the downgradient, confined, arsenic-rich ground water. High ??18O[SO4] values there cannot be due to aeration by atmospheric oxygen, but may arise from reoxidation of reduced SO4 products. The enrichment factors of ??18O in SO4 compared to H2O, + 7.2 to + 15.5???, in the Kelly's Cove ground water and the negligible 34S enrichment is very similar to those derived from experimental data of anaerobic sulfide oxidation in the presence of Mn and Fe oxides. Sea level at the Kelly's Cove watershed was approximately 80??m above present sea level about 13 000??years before present, imposing reducing conditions on that area of the watershed. Sea level dropped approximately 60??m below present sea level about 11 000??years before present, allowing for possible oxidation of sulfide minerals and precipitation of arsenic in ferric oxyhydroxides during aeration of the ground-water system. Under present redox conditions, there is evidence that bacteria reduction of ferric oxyhydroxides releases arsenic. The fractionation of 18O in the SO4 during anaerobic oxidation of sulfide in the presence of Mn and Fe oxides and subsequent release of arsenic during Mn and Fe oxide reduction may explain the relationship between high arsenic concentrations and elevated 18O[SO4] at Kelly's Cove. ?? 2007 Elsevier B.V. All rights reserved.

Chemical Geology↗

USGS2009

Changing sources of strontium to soils and ecosystems across the Hawaiian Islands

Strontium isotope ratios assist ecosystem scientists in constraining the sources of alkaline earth elements, but their interpretation can be difficult because of complexities in mineral weathering and in the geographical and environmental controls on elemental additions and losses. Hawaii is a "natural laboratory" where a number of important biogeochemical variables have either limited ranges or vary in systematic ways, providing a unique opportunity to understand the impact of time, climate, and atmospheric inputs on the evolution of base cation sources to ecosystems. There are three major sources of strontium (Sr) to these ecosystems, each with distinct isotopic compositions: basalt lava, Asian dust, and rainfall. We present Sr isotope and concentration data on both bulk soil digests and NH 4 Ac extracts from soil profiles covering a wide range of environments and substrate ages. Bulk soil material from dry climates and/or young substrate ages with > 80????g g - 1 Sr retain basalt-like Sr isotopic signatures, whereas those with Sr concentrations < 80????g g - 1 can have isotope signatures that range from basalt-like values to the more radiogenic values associated with continental dust. Although both dust accumulation and lava weathering are time- and rainfall-dependent, the overall concentration of Sr drops with increasing leaching even as quartz and mica derived from continental dust sources increase to > 40% by mass. At elevated dust levels, lava-derived Sr is low and dust-derived Sr is the dominant control of 87 Sr/ 86 Sr in bulk soils; however, 87 Sr/ 86 Sr of NH 4 Ac-extractable Sr largely reflects atmospheric deposition of marine aerosol in these situations. Overall, whole-soil Sr isotope values are controlled by complex interactions between Sr provided by lava weathering but partially lost by leaching, and Sr provided by dust but held in more resistant minerals. The isotopic composition of NH 4 Ac-extractable Sr and of the biota is controlled by lava weathering and rainfall contribution of Sr with only minor contributions from radiogenic dust sources. ?? 2009 Elsevier B.V.

Chemical Geology↗

USGS2010

River solute fluxes reflecting active hydrothermal chemical weathering of the Yellowstone Plateau Volcanic Field, USA

In the past few decades numerous studies have quantified the load of dissolved solids in large rivers to determine chemical weathering rates in orogenic belts and volcanic areas, mainly motivated by the notion that over timescales greater than ~100kyr, silicate hydrolysis may be the dominant sink for atmospheric CO2, thus creating a feedback between climate and weathering. Here, we report the results of a detailed study during water year 2007 (October 1, 2006 to September 30, 2007) in the major rivers of the Yellowstone Plateau Volcanic Field (YPVF) which hosts Earth's largest "restless" caldera and over 10,000 thermal features. The chemical compositions of rivers that drain thermal areas in the YPVF differ significantly from the compositions of rivers that drain non-thermal areas. There are large seasonal variations in river chemistry and solute flux, which increases with increasing water discharge. The river chemistry and discharge data collected periodically over an entire year allow us to constrain the annual solute fluxes and to distinguish between low-temperature weathering and hydrothermal flux components. The TDS flux from Yellowstone Caldera in water year 2007 was 93t/km2/year. Extensive magma degassing and hydrothermal interaction with rocks accounts for at least 82% of this TDS flux, 83% of the cation flux and 72% of the HCO3- flux. The low-temperature chemical weathering rate (17t/km2/year), calculated on the assumption that all the Cl- is of thermal origin, could include a component from low-temperature hydrolysis reactions induced by CO2 ascending from depth rather than by atmospheric CO2. Although this uncertainty remains, the calculated low-temperature weathering rate of the young rhyolitic rocks in the Yellowstone Caldera is comparable to the world average of large watersheds that drain also more soluble carbonates and evaporates but is slightly lower than calculated rates in other, less-silicic volcanic regions. Long-term average fluxes at Yellowstone are likely ~20% higher than those in the abnormally dry water year 2007, but the protocol used in this study can be easily adaptable to track future changes in low-temperature weathering and hydrothermal flux components, which could provide better monitoring of magmatic unrest. ?? 2010.

Chemical Geology↗

USGS2013

Mass fractionation of noble gases in synthetic methane hydrate: Implications for naturally occurring gas hydrate dissociation

As a consequence of contemporary or longer term (since 15 ka) climate warming, gas hydrates in some settings may presently be dissociating and releasing methane and other gases to the ocean-atmosphere system. A key challenge in assessing the impact of dissociating gas hydrates on global atmospheric methane is the lack of a technique able to distinguish between methane recently released from gas hydrates and methane emitted from leaky thermogenic reservoirs, shallow sediments (some newly thawed), coal beds, and other sources. Carbon and deuterium stable isotopic fractionation during methane formation provides a first-order constraint on the processes (microbial or thermogenic) of methane generation. However, because gas hydrate formation and dissociation do not cause significant isotopic fractionation, a stable isotope-based hydrate-source determination is not possible. Here, we investigate patterns of mass-dependent noble gas fractionation within the gas hydrate lattice to fingerprint methane released from gas hydrates. Starting with synthetic gas hydrate formed under laboratory conditions, we document complex noble gas fractionation patterns in the gases liberated during dissociation and explore the effects of aging and storage (e.g., in liquid nitrogen), as well as sampling and preservation procedures. The laboratory results confirm a unique noble gas fractionation pattern for gas hydrates, one that shows promise in evaluating modern natural gas seeps for a signature associated with gas hydrate dissociation.

Chemical Geology↗

USGS2021

Noble gas signatures constrain oil-field water as the carrier phase of hydrocarbons occurring in shallow aquifers in the San Joaquin Basin, USA

Noble gases record fluid interactions in multiphase subsurface environments through fractionation processes during fluid equilibration. Water in the presence of hydrocarbons at the subsurface acquires a distinct elemental signature due to the difference in solubility between these two fluids. We find the atmospheric noble gas signature in produced water is partially preserved after hydrocarbons production and water disposal to unlined ponds at the surface. This signature is distinct from meteoric water and can be used to trace oil-field water seepage into groundwater aquifers. We analyse groundwater ( n = 30) and fluid disposal pond ( n = 2) samples from areas overlying or adjacent to the Fruitvale, Lost Hills, and South Belridge Oil Fields in the San Joaquin Basin, California, USA. Methane (2.8 × 10 −7 to 3 × 10 −2 cm 3 STP/cm 3 ) was detected in 27 of 30 groundwater samples. Using atmospheric noble gas signatures, the presence of oil-field water was identified in 3 samples, which had equilibrated with thermogenic hydrocarbons in the reservoir. Two (of the three) samples also had a shallow microbial methane component, acquired when produced water was deposited in a disposal pond at the surface. An additional 6 samples contained benzene and toluene, indicative of interaction with oil-field water; however, the noble gas signatures of these samples are not anomalous. Based on low tritium and 14 C contents (≤ 0.3 TU and 0.87–6.9 pcm, respectively), the source of oil-field water is likely deep, which could include both anthropogenic and natural processes. Incorporating noble gas analytical techniques into the groundwater monitoring programme allows us to 1) differentiate between thermogenic and microbial hydrocarbon gas sources in instances when methane isotope data are unavailable, 2) identify the carrier phase of oil-field constituents in the aquifer (gas, oil-field water, or a combination), and 3) differentiate between leakage from a surface source (disposal ponds) and from the hydrocarbon reservoir (either along natural or anthropogenic pathways such as faulty wells).

California↗

USGS2022

Towards a holistic sulfate-water-O2 triple oxygen isotope systematics

Triple oxygen isotope (∆ 17 O with δ 18 O) signals of H 2 O and O 2 found in sulfate of oxidative weathering origin offer promising constraints on modern and ancient weathering, hydrology, atmospheric gas concentrations, and bioproductivity. However, interpretations of the sulfate-water-O 2 system rely on assuming fixed oxygen-isotope fractionations between sulfate and water, which, contrastingly, are shown to vary widely in sign and amplitude. Instead, here we anchor sulfate-water-O 2 triple oxygen isotope systematics on the homogeneous composition of atmospheric O 2 with empirical constraints and modeling. Our resulting framework does not require a priori assumptions of the O 2 - versus H 2 O‑oxygen ratio in sulfate and accounts for the signals of mass-dependent and mass-independent fractionation in the ∆ 17 O and δ 18 O of sulfate's O 2 ‑oxygen source. Within this framework, new ∆ 17 O measurements of sulfate constrain ~2.3 Ga Paleoproterozoic gross primary productivity to between 6 and 160 times present-day levels, with important implications for the biological carbon cycle response to high CO 2 concentrations prevalent on the early Earth.

Chemical Geology↗

USGS2010

The carbon budget of the northern cryosphere region

The northern cryosphere is undergoing substantial warming of permafrost and loss of sea ice. Release of stored carbon to the atmosphere in response to this change has the potential to affect the global climate system. Studies indicate that the northern cryosphere has been not only a substantial sink for atmospheric CO 2 in recent decades, but also an important source of CH 4 because of emissions from wetlands and lakes. Analyses suggest that the sensitivity of the carbon cycle of the region over the 21st Century is potentially large, but highly uncertain because numerous pathways of response will be affected by warming. Further research should focus on sensitive elements of the carbon cycle such as the consequences of increased fire disturbance, permafrost degradation, and sea ice loss in the northern cryosphere region.

Current Opinion in Environmental Sustainability↗

USGS2013

Nature's refineries — Metals and metalloids in arc volcanoes

Chemical data for fumaroles and for atmospheric gas and ash plumes from active arc volcanoes provide glimpses of the rates of release of metal and metalloids, such as Tl and Cd, from shallow and mid-crust magmas. Data from copper deposits formed in ancient volcanoes at depths of up to about 1500 m in the fractures below paleo-fumaroles, and at around 2000–4000 m in association with sub-volcanic intrusions (porphyry copper deposits) provide evidence of sub-surface deposition of Cu–Au–Ag–Mo and a range of other minor elements including Te, Se, As and Sb. These deposits, or ‘sinks’, of metals consistently record sustained histories of magmatic gas streaming through volcanic systems interspersed by continuing intrusive and eruptive activity. Here we integrate data from ancient and modern volcanic systems and show that the fluxes of metals and metalloids are controlled by a) the maintenance of fracture permeability in the stressed crust below volcanoes and b) the chemical processes that are triggered as magmatic gas, initially undersaturated with metals and metalloids, expands from lithostatic to very low pressure conditions through fracture arrays. The recognition of gas streaming may also account for the phenomenon of ‘excess degassing’, and defines an integral, but generally understated, component of active volcanic systems – a volcanic gas core – that is likely to be integral to the progression of eruptions to Plinean state. Destabilization of solvated molecular metal and metalloid species in magmatic gas mixtures and changes in their redox state are triggered, as it expands to the surface by abrupt pressure drops, or throttles' in the fracture array that guides expansion to the surface. The electronically harder, low electronegativity metals, such as copper and iron, deposit rapidly in response to expansion followed more slowly by arsenic with antimony as sulfosalts. Heavy, large radius, softer elements such as bismuth, lead, and thallium along with cadmium are strongly fractionated along the way, eventually venting their excess along with SO 2 , CO 2 , and other components of the carrier gas, into the atmosphere. These elements, many of which are toxic, may also be dispersed by mixing with groundwater in the permeable crust below volcanoes and generate potential health risks due to Hg, As, and Se contamination of drinking water resources.

Earth-Science Reviews↗

USGS2024

Dust in the Critical Zone: North American case studies

The dust cycle facilitates the exchange of particles among Earth's major systems, enabling dust to traverse ecosystems, cross geographic boundaries, and even move uphill against the natural flow of gravity. Dust in the atmosphere is composed of a complex and ever-changing mixture that reflects the evolving human footprint on the landscape. The emission, transport, and deposition of dust interacts with and connects Critical Zone processes at all spatial and temporal scales. Landscape properties, land use, and climatic factors influence the wind erosion of soil and nutrient loss, which alters the long-term ecological dynamics at erosional locations. Once in the atmosphere, dust particles influence the amount of solar radiation reaching Earth, and interact with longwave (terrestrial) radiation, with cascading effects on the climate system. Finally, the wet and dry deposition of particles influences ecosystem structure, composition, and function over both short and long-term scales. Tracking dust particles from source to sink relies on monitoring and measurement of the geochemical composition and size distribution of the particles, space-borne and ground-based remote sensing, and dust modeling. Dust is linked to human systems via land use and policies that contribute to dust emissions and the health-related consequences of particulate loads and composition. Despite the significant influence dust has in shaping coupled natural-human systems, it has not been considered a key component of the Critical Zone. Here, we demonstrate that dust particles should be included as a key component of the Critical Zone by outlining how dust interacts with and shapes Earth System processes from generation, through transport, to deposition. We synthesize current understanding from global research and identify critical data and knowledge gaps while showcasing case studies from North America.

Earth-Science Reviews↗

USGS2019

Carbon storage potential in a recently created brackish marsh in eastern North Carolina, USA

Carbon (C) sequestration through accumulated plant biomass and storage in soils can potentially make wetland ecosystems net C sinks. Here, we collected GHG flux, plant biomass, and litter decomposition data from three distinct vegetation zones ( Spartina alterniflora , Juncus roemerianus and Spartina patens ) on a 7-year-old created brackish marsh in North Carolina, USA, and integrate these data into an overall C mass balance budget. The marsh fixed an average of 1.85 g C m −2 day −1 through plant photosynthesis. About 41–46% of the fixed C remained in plants, while 18.4% of the C was decomposed and released back to the atmosphere as CO 2 and CH 4 , and 8.6–13.2% of the decomposed C was stored as soil C. In all, this created marsh sequestered 28.7–44.7 Mg CO 2 year −1 across the 14 ha marsh. Because the brackish marsh emitted only small amounts of CH 4 and N 2 O, the CO 2 equivalent emission of the marsh was −0.87 to −0.56 g CO 2-eq m −2 day −1 , indicating the marsh has a net effect in reducing GHGs to the atmosphere and contributes to cooling. However, resultant CO 2 credit (through the increment of soil C) would be worth only $30.76–$47.90 USD per hectare annually, or $431–$671 per year for the project, which, coupled with other enhanced ecosystem services, could provide landowners with some additional economic incentive for future creation projects. Nevertheless, C mass balance determinations and radiative cooling metrics showed promise in demonstrating the potential of a young created brackish marsh to act as a net carbon sink.

North Carolina↗

USGS2011

Estimating aboveground forest biomass carbon and fire consumption in the U.S. Utah High Plateaus using data from the Forest Inventory and Analysis program, Landsat, and LANDFIRE

The concentrations of CO 2 and other greenhouse gases in the atmosphere have been increasing and greatly affecting global climate and socio-economic systems. Actively growing forests are generally considered to be a major carbon sink, but forest wildfires lead to large releases of biomass carbon into the atmosphere. Aboveground forest biomass carbon (AFBC), an important ecological indicator, and fire-induced carbon emissions at regional scales are highly relevant to forest sustainable management and climate change. It is challenging to accurately estimate the spatial distribution of AFBC across large areas because of the spatial heterogeneity of forest cover types and canopy structure. In this study, Forest Inventory and Analysis (FIA) data, Landsat, and Landscape Fire and Resource Management Planning Tools Project (LANDFIRE) data were integrated in a regression tree model for estimating AFBC at a 30-m resolution in the Utah High Plateaus. AFBC were calculated from 225 FIA field plots and used as the dependent variable in the model. Of these plots, 10% were held out for model evaluation with stratified random sampling, and the other 90% were used as training data to develop the regression tree model. Independent variable layers included Landsat imagery and the derived spectral indicators, digital elevation model (DEM) data and derivatives, biophysical gradient data, existing vegetation cover type and vegetation structure. The cross-validation correlation coefficient ( r value) was 0.81 for the training model. Independent validation using withheld plot data was similar with r value of 0.82. This validated regression tree model was applied to map AFBC in the Utah High Plateaus and then combined with burn severity information to estimate loss of AFBC in the Longston fire of Zion National Park in 2001. The final dataset represented 24 forest cover types for a 4 million ha forested area. We estimated a total of 353 Tg AFBC with an average of 87 MgC/ha in the Utah High Plateaus. We also estimated that 8054 Mg AFBC were released from 2.24 km 2 burned forest area in the Longston fire. These results demonstrate that an AFBC spatial map and estimated biomass carbon consumption can readily be generated using existing database. The methodology provides a consistent, practical, and inexpensive way for estimating AFBC at 30-m resolution over large areas throughout the United States.

Ecological Indicators↗